JP2008163944A - Reforming system for partial co2 recovery type cycle plant - Google Patents

Reforming system for partial co2 recovery type cycle plant Download PDF

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JP2008163944A
JP2008163944A JP2007333398A JP2007333398A JP2008163944A JP 2008163944 A JP2008163944 A JP 2008163944A JP 2007333398 A JP2007333398 A JP 2007333398A JP 2007333398 A JP2007333398 A JP 2007333398A JP 2008163944 A JP2008163944 A JP 2008163944A
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steam
reformate
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Ke Liu
ケ・リュ
Michael John Bowman
マイケル・ジョン・ボウマン
Stephen Duane Sanborn
スティーブン・ドュエイン・サンボーン
Andrei T Evulet
アンドレイ・トリスタン・エヴュレット
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    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
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    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
    • C01B2203/0227—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step
    • C01B2203/0233—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step the reforming step being a steam reforming step
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    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
    • C01B2203/0465—Composition of the impurity
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    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/08—Methods of heating or cooling
    • C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
    • C01B2203/0833—Heating by indirect heat exchange with hot fluids, other than combustion gases, product gases or non-combustive exothermic reaction product gases
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    • C01B2203/80—Aspect of integrated processes for the production of hydrogen or synthesis gas not covered by groups C01B2203/02 - C01B2203/1695
    • C01B2203/84—Energy production
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Abstract

<P>PROBLEM TO BE SOLVED: To reduce the amount of carbon dioxide discharged to the atmosphere from a combined cycle plant. <P>SOLUTION: The plant is structured by including: a reforming device 12 structured to receive a fuel 18 such as a natural gas to generate a hydrogen-concentrated flow; a combustion system comprising a gas turbine 54 structured to burn the hydrogen-concentrated flow to generate power and an exhaust gas flow; and a heat recovery device 80 to recover heat from the exhaust gas flow to recycle and return the recovered heat to the reforming device. <P>COPYRIGHT: (C)2008,JPO&INPIT

Description

本発明は、部分的ＣＯ２回収式サイクルプラントのための改質システム及び方法に関する。 The present invention relates to a reforming system and method for a partial CO 2 capture cycle plant.

いわゆる温室効果ガスの１種である二酸化炭素（ＣＯ２）は、炉及び発電所での化石燃料の燃焼中に生成する。近年の研究で、ＣＯ２及びメタン（ＣＨ４）や窒素酸化物（Ｎ２Ｏ）のような他の温室効果ガスの排出が、気候変動に重大な影響を及ぼしかねないことが判明している。ＣＯ２その他の温室効果ガスの排出に少なくとも部分的に起因する気候変動の予想は、国際的な関心事となり、京都議定書などの国際協定に結びついている。 Carbon dioxide (CO 2 ), a so-called greenhouse gas, is produced during the burning of fossil fuels in furnaces and power plants. Recent research has shown that emissions of CO 2 and other greenhouse gases such as methane (CH 4 ) and nitrogen oxides (N 2 O) can have a significant impact on climate change. . Anticipation of climate change due, at least in part, to emissions of CO 2 and other greenhouse gases has become an international concern and has been linked to international agreements such as the Kyoto Protocol.

全国的及び国際的な関心事のため、電力生産者は、発電プラントで発生するＣＯ２レベルを減らすことを試みている。多くの最新発電プラントは、天然ガスで燃焼する複合サイクルプラント又は「ＮＧＣＣ」プラントである。これらのプラントは、石炭を燃焼させる発電プラントよりも格段に少量のＣＯ２しか発生しないが、常に厳しくなる排出基準を満たすのは依然として困難である。最近、ヨーロッパの政策立案者は、特定の発電所が年間に排出できるＣＯ２の最大割当量の作成を提案した。この割当量を超えるＣＯ２排出は、過剰量について「炭素税」を支払われなければならないと提案されている。実際、スウェーデンには、既に所々で炭素税がある。同様に、ノルウェー、フィンランド及びオランダでも、最近炭素税が制定されている。同様な炭素税の提案は、大気環境基準を厳しくすることに決めた米国のカリフォルニアその他の州で議論されている。 For national and international concern, power producers have attempted to reduce the CO 2 level generated by the power plant. Many modern power plants are combined cycle plants or “NGCC” plants that burn with natural gas. These plants produce significantly less CO 2 than power plants that burn coal, but it is still difficult to meet ever-stricter emission standards. Recently, European policymakers have proposed creating a maximum CO 2 quota that a particular power plant can emit annually. It is proposed that CO 2 emissions exceeding this quota must be paid a “carbon tax” for the excess. In fact, Sweden already has carbon taxes in places. Similarly, carbon taxes have recently been enacted in Norway, Finland and the Netherlands. Similar carbon tax proposals are being discussed in California and other states in the United States that have decided to tighten air quality standards.

既存の発電プラントは、水蒸気メタン改質（ＳＭＲ）、自己熱交換式改質（ＡＴＲ）及び触媒部分酸化（ＣＰＯ）を利用して、天然ガス（ＮＧ）を、ガスタービン発生装置用の水素及び一酸化炭素からなる合成ガス又はリフォーメート、並びにアンモニア製造又は精製装置用の水素に転化することができる。リフォーメートの使用でＮＯｘの排出を減らすことができるが、天然ガス（ＮＧ）の改質反応、並びに発電に要する燃焼は、大量の二酸化炭素を発生しかねない。ＮＧ全体の改質に必要とされる改質装置は、非常に大規模で広大である必要があろう。さらに、ＳＭＲ改質装置を使用した場合、改質装置の炉側を２６００°Ｆもの高温で稼動する必要があろう。かかる温度では、ＳＭＲ改質装置を高価な耐熱合金で作る必要がある。おそらく、さらに重大な障害は、かかる改質装置で発生した大量の二酸化炭素を回収することである。過剰ＣＯ２排出を回収するには多量の燃料が必要とされるので、かかる大量の二酸化炭素の回収は費用がかかり、プラント全体の効率が下がる。このように、厳しさを増しつつあるＣＯ２排出基準を順守する能力を既存の発電プラントに与えるには、多大な資本投下が必要とされるであろう。
米国特許第６２２３５１９号明細書 米国特許出願公開第２００６／０１３７２４６号明細書 米国特許出願公開第２００５／０１７６８３１号明細書 Existing power plants utilize steam methane reforming (SMR), self heat exchange reforming (ATR) and catalytic partial oxidation (CPO) to convert natural gas (NG) to hydrogen for gas turbine generators and It can be converted to synthesis gas or reformate consisting of carbon monoxide and hydrogen for ammonia production or purification equipment. Although it is possible to reduce the NO x emissions in the use of reformate, reforming reaction of natural gas (NG), and combustion required for power generation, could generate a significant amount of carbon dioxide. The reformer required for reforming the entire NG will need to be very large and vast. Furthermore, if an SMR reformer is used, the furnace side of the reformer will need to operate at temperatures as high as 2600 ° F. At such temperatures, the SMR reformer must be made of an expensive heat resistant alloy. Perhaps a more serious obstacle is the recovery of large amounts of carbon dioxide generated in such reformers. Since a large amount of fuel is required to recover excess CO 2 emissions, the recovery of such a large amount of carbon dioxide is expensive and reduces the efficiency of the entire plant. Thus, it gives the ability to comply with CO 2 emission standards are becoming increasingly severe in existing power plants, would significant capital investment is required.
US Pat. No. 6,223,519 US Patent Application Publication No. 2006/0137246 US Patent Application Publication No. 2005/0176831

そこで、ＮＧを転化させ、生成ＣＯ２の一部を回収するための安価な低温改質装置を利用することができる発電プラントに対するニーズが存在する。かかるシステムでは、低温で稼動し、効率を高めるためリサイクル流を使用し、プラントの年間割当量を超えて発生したＣＯ２排出だけを回収して高価な炭素税を避けることによって、資本及び運転費用が低減する。さらに、既存のＮＧＣＣ発電プラントを改造してこのようなシステムを組み込むことができれば有益である。 Therefore, there is a need for a power plant that can convert an NG and use an inexpensive low-temperature reformer for recovering a part of the produced CO 2 . Such systems operate at low temperatures, use recycle streams to increase efficiency, and recover capital and operating costs by collecting only CO 2 emissions that exceed the annual quota of the plant and avoiding expensive carbon taxes. Is reduced. Furthermore, it would be beneficial if an existing NGCC power plant could be modified to incorporate such a system.

本願では、二酸化炭素を部分的に回収する天然ガス複合サイクルシステム並びにその稼働方法について開示する。一実施形態では、複合サイクルシステムは、約８００℃未満の温度で稼動して、第１燃料と水蒸気とを含む混合燃料流を改質して第１リフォーメート流を生成するように構成されたプレ−水蒸気−メタン−改質装置を含む改質装置ユニット、第１リフォーメート流中の一酸化炭素を二酸化炭素に転化させて第２リフォーメート流を生成するように構成された水−ガス−転化反応器を含む転化反応ユニット、第２リフォーメート流から二酸化炭素を除去し、二酸化炭素流及び第３リフォーメート流を生成するように構成された二酸化炭素除去ユニットであって、第１燃料中に含まれる炭素の約５０％未満を二酸化炭素として回収する二酸化炭素除去ユニット、第３リフォーメート流及び第２燃料の混合物を受け入れて電力及び排気ガス流を発生させるように構成されたガスタービンユニットであって、排気ガス流が混合燃料流を改質するための熱を供給するガスタービンユニット、及び排気ガス流を受け入れるように構成された水蒸気発生器ユニットであって、排気ガス流の熱を水流に伝達して冷却排気ガス流及び水蒸気タービンのための水蒸気及び混合燃料流を生成する水蒸気発生器ユニットを備える。   The present application discloses a natural gas combined cycle system that partially recovers carbon dioxide and an operation method thereof. In one embodiment, the combined cycle system is configured to operate at a temperature less than about 800 ° C. to reform a mixed fuel stream that includes a first fuel and steam to produce a first reformate stream. A reformer unit including a pre-steam-methane-reformer, water-gas configured to convert carbon monoxide in the first reformate stream to carbon dioxide to produce a second reformate stream A conversion reaction unit including a conversion reactor, a carbon dioxide removal unit configured to remove carbon dioxide from a second reformate stream to produce a carbon dioxide stream and a third reformate stream, wherein the carbon dioxide removal unit is in a first fuel. Accepts a mixture of carbon dioxide removal unit, third reformate stream and second fuel that recovers less than about 50% of the carbon contained in as carbon dioxide and generates electric power and exhaust gas stream A gas turbine unit configured to allow the exhaust gas stream to supply heat for reforming the mixed fuel stream, and a steam generator unit configured to receive the exhaust gas stream And a steam generator unit for transferring heat of the exhaust gas stream to the water stream to generate a cooled exhaust gas stream and steam and a mixed fuel stream for the steam turbine.

部分的に二酸化炭素を回収して発電する方法は、プレ−水蒸気−メタン−改質装置で第１燃料と水蒸気とを含む混合燃料流を改質して水素と一酸化炭素と水蒸気とを含む第１リフォーメート流を生成させ、水−ガス−転化反応器で水蒸気及び第１リフォーメート流中の一酸化炭素を二酸化炭素と水素とを含む第２リフォーメート流に転化させ、二酸化炭素除去ユニットで第２リフォーメート流から二酸化炭素を除去して二酸化炭素流及び第３リフォーメート流を生成させて、第１燃料中に含まれる炭素の約５０％未満を二酸化炭素として回収し、ガスタービンユニットで第３リフォーメート流と第２燃料流との混合物を燃焼させて電力を発生させ、排気ガス流を生成させ、熱回収水蒸気発生器で排気ガス流中の熱を利用して水蒸気を発生させ、水蒸気で電力を発生させるとともに第１燃料との混合燃料流を生成させることを含む。   A method of generating electricity by partially recovering carbon dioxide includes hydrogen, carbon monoxide, and steam by reforming a mixed fuel stream including a first fuel and steam in a pre-steam-methane-reformer. A first reformate stream is generated, and in a water-gas-conversion reactor, water vapor and carbon monoxide in the first reformate stream are converted to a second reformate stream containing carbon dioxide and hydrogen, and a carbon dioxide removal unit And removing carbon dioxide from the second reformate stream to generate a carbon dioxide stream and a third reformate stream, and recovering less than about 50% of the carbon contained in the first fuel as carbon dioxide, a gas turbine unit To burn the mixture of the third reformate stream and the second fuel stream to generate electric power, to generate an exhaust gas stream, and to generate steam by using heat in the exhaust gas stream with a heat recovery steam generator. It comprises generating the mixed fuel stream to the first fuel with generating electric power with steam.

別の実施形態では、複合サイクルシステムは、熱回収水蒸気発生器を含む複合ユニットであって、熱回収水蒸気発生器が２以上のステージを含んでいて、第１ステージがプレ−水蒸気−メタン−改質装置を備えており、該プレ−水蒸気−メタン−改質装置が、約８００℃未満の温度で稼動し、高温ガスタービン排気ガス流からの熱を利用して混合燃料流を改質して第１リフォーメート流を生成するように構成されており、第２ステージで、排気ガス流からの熱を利用して水蒸気を生成させる複合ユニット、第１リフォーメート流中の一酸化炭素を二酸化炭素に転化させて第２リフォーメート流を生成するように構成された、水−ガス−転化反応器を含む転化反応ユニット、第２リフォーメート流から二酸化炭素を除去て二酸化炭素流と第３リフォーメート流とを生成するように構成された二酸化炭素除去ユニットであって、第１燃料中に含まれる炭素の約５０％未満を二酸化炭素として回収する二酸化炭素除去ユニット、及び第２燃料及び第３リフォーメート流を受け入れ、電力及び排気ガス流を発生するように構成されたガスタービンユニットを備える。   In another embodiment, the combined cycle system is a combined unit including a heat recovery steam generator, wherein the heat recovery steam generator includes two or more stages, and the first stage is pre-steam-methane-modified. The pre-steam-methane-reformer operates at a temperature of less than about 800 ° C. and utilizes the heat from the hot gas turbine exhaust gas stream to reform the mixed fuel stream. A composite unit configured to generate a first reformate stream and generating water vapor using heat from the exhaust gas stream in the second stage, and carbon monoxide in the first reformate stream to carbon dioxide A conversion reaction unit comprising a water-gas-conversion reactor configured to convert to a second reformate stream, removing carbon dioxide from the second reformate stream and removing the carbon dioxide stream and the third reformate stream. A carbon dioxide removal unit configured to generate a formate stream, wherein the carbon dioxide removal unit recovers less than about 50% of the carbon contained in the first fuel as carbon dioxide, and the second fuel and the third fuel. A gas turbine unit is provided that is configured to receive the reformate stream and generate a power and exhaust gas stream.

以下、図面を参照するが、図面では同様の要素には同様の符号を付した。   In the following, reference is made to the drawings, in which like elements are given like reference numerals.

本願では、プレ−水蒸気−メタン−改質装置（ＳＭＲ）及び部分的ＣＯ２回収ユニットを利用する複合サイクル発電システム及び方法について開示される。複合サイクルシステムは、熱回収を利用して、水蒸気の生成のためにガスタービン排気ガス中のエネルギーを回収することによって、Ｒａｎｋｉｎｅ（水蒸気タービン）とＢｒａｙｔｏｎ（ガスタービン）の熱力学的サイクルを組み合わせる。従来の改質装置を使用する従来技術の複合サイクルプラントと対比すると、本願で開示するシステム及び方法では、特定の許容範囲を超えるＣＯ２排出量の回収に天然ガスの（ＮＧ）の一部のみを改質するため低温プレ−ＳＭＲを用いるという利点がある。従来のＳＭＲでは、メタンを水素に完全に転化させるには反応を高温、例えば１０００℃超の温度で起こさなければならない。しかし、本願で開示するプレ−ＳＭＲでは、反応温度は、約５５０℃〜約８００℃、具体的には約６００℃〜約７５０℃、さらに具体的には６５０℃である。燃料流中の炭素の約５０％未満を回収することが望まれるので、プレ−ＳＭＲで必要とされるのはメタンから水素及び一酸化炭素への７０％以下の転化効率のみである。さらに、本願で開示するシステムは、プレ−ＳＭＲへ送り込まれるＮＧ及び水蒸気を予熱するため、プレ−ＳＭＲ及び水−ガス−転化（ＷＧＳ）反応器から出るリフォーメートの熱の回収に再生式熱交換器を用いてシステム全体の効率を高める。また、プレ−ＳＭＲは、既存の熱回収水蒸気発生器（ＨＲＳＧ）を改造して組み込むことができ、分離したＳＭＲユニットに伴う追加の資本コストもスペースも必要とせずに、本発明のシステムの利益を得ることができる。 The present application discloses a combined cycle power generation system and method that utilizes a pre-steam-methane-reformer (SMR) and a partial CO 2 capture unit. A combined cycle system utilizes heat recovery to combine Rankine (steam turbine) and Brayton (gas turbine) thermodynamic cycles by recovering energy in the gas turbine exhaust for steam generation. In contrast to prior art combined cycle plants that use conventional reformers, the systems and methods disclosed herein provide only a portion of natural gas (NG) for the recovery of CO 2 emissions that exceed a specified tolerance. There is an advantage that a low temperature pre-SMR is used to improve the temperature. In conventional SMR, the reaction must occur at a high temperature, for example, above 1000 ° C., to completely convert methane to hydrogen. However, in the pre-SMR disclosed herein, the reaction temperature is about 550 ° C to about 800 ° C, specifically about 600 ° C to about 750 ° C, more specifically 650 ° C. Since it is desired to recover less than about 50% of the carbon in the fuel stream, only a conversion efficiency of less than 70% from methane to hydrogen and carbon monoxide is required in pre-SMR. Further, the system disclosed herein regenerative heat exchange to recover the heat of reformate exiting the pre-SMR and water-gas-conversion (WGS) reactors to preheat NG and water vapor fed to the pre-SMR. To increase the efficiency of the entire system. The pre-SMR can also be retrofitted to an existing heat recovery steam generator (HRSG), without the additional capital cost and space associated with a separate SMR unit, and the benefits of the system of the present invention. Can be obtained.

本明細書で用いる用語は、説明のためのものであり、限定を目的としたものではない。本明細書に記載した構造及び機能の詳細は、限定的に解釈すべきではなく、特許請求の範囲の基礎として当業者が本発明を様々に利用できるように教示するための代表的な情報源である。さらに、本明細書で用いる「第１」、「第２」などの用語は、順序又は重要性を意味するものではなく、ある要素を、他のものから区別するために用いるものであり、単数形で記載したものであっても、量を限定するものではなく、そのものが１以上存在することを意味する。量について用いる修飾語「約」は、標記の数値を含むだけでなく、文脈に応じた意味を有する（例えば、特定の量の測定に付随する誤差を含む。）。さらに、特定の成分の量又は測定値に関する範囲はすべて、上下限を含むとともに、独立に結合できる。   The terminology used herein is for the purpose of description and is not intended to be limiting. The details of structure and function described herein should not be construed as limiting, but are representative sources for teaching those skilled in the art to use the present invention in various ways as a basis for the claims. It is. Furthermore, terms such as “first”, “second”, etc., as used herein do not imply order or importance, but are used to distinguish one element from another, Even if it is described in the form, it does not limit the amount, but means that one or more of them exist. The modifier "about" used for a quantity not only includes the indicated numerical value, but also has a contextual meaning (eg, includes errors associated with the measurement of a particular quantity). Further, all ranges relating to the amount or measurement of a particular component include upper and lower limits and can be combined independently.

図１は、発電してＣＯ２排出を回収するための例示的なＮＧＣＣ発電システム１０を表す。発電システム１０は、プレ−ＳＭＲ１４を有する改質装置ユニット１２及び熱交換器１６を備える。改質装置ユニット１２は、第１燃料１８と水蒸気２０を混合燃料流２２として受け入れて、一酸化炭素、水素、未転化燃料及び水蒸気からなる第１リフォーメート流２４を生成する。熱交換器１６は、第１リフォーメート流２４からの熱を混合燃料流２２に伝達し、冷却第１リフォーメート流２６と加熱混合燃料流２８とを生成する。発電システム１０は、転化反応ユニット３０をさらに備える。冷却第１リフォーメート流２６は、転化反応ユニット３０に送られ、第１リフォーメート流２６中の一酸化炭素（ＣＯ）と水蒸気はＷＧＳ反応器３２で二酸化炭素と水素に転化される。第２リフォーメート流３４はＷＧＳ反応器を出て熱交換器３６に入る。熱交換器３６は、第２リフォーメート流３４から熱を第１燃料１８に伝達して、冷却第２リフォーメート流３８と加熱第１燃料１８とを生成する。冷却第２リフォーメート流３８はＣＯ２除去ユニット４０に送られる。ＣＯ２除去ユニット４０はアミン吸収塔４２と再生塔４４とを備えていて、冷却第２リフォーメート流２８から二酸化炭素を除去して、二酸化炭素流４６と、水素、一酸化炭素及び未転化燃料を含む第３リフォーメート流４８とを生成する。 FIG. 1 represents an exemplary NGCC power generation system 10 for generating power and recovering CO 2 emissions. The power generation system 10 includes a reformer unit 12 having a pre-SMR 14 and a heat exchanger 16. The reformer unit 12 receives the first fuel 18 and the steam 20 as a mixed fuel stream 22 and produces a first reformate stream 24 composed of carbon monoxide, hydrogen, unconverted fuel, and steam. The heat exchanger 16 transfers heat from the first reformate stream 24 to the mixed fuel stream 22 to produce a cooled first reformate stream 26 and a heated mixed fuel stream 28. The power generation system 10 further includes a conversion reaction unit 30. The cooled first reformate stream 26 is sent to the conversion reaction unit 30 where carbon monoxide (CO) and water vapor in the first reformate stream 26 are converted to carbon dioxide and hydrogen in the WGS reactor 32. Second reformate stream 34 exits the WGS reactor and enters heat exchanger 36. The heat exchanger 36 transfers heat from the second reformate stream 34 to the first fuel 18 to produce a cooled second reformate stream 38 and a heated first fuel 18. The cooled second reformate stream 38 is sent to the CO 2 removal unit 40. The CO 2 removal unit 40 includes an amine absorption tower 42 and a regeneration tower 44, which removes carbon dioxide from the cooled second reformate stream 28 to produce a carbon dioxide stream 46, hydrogen, carbon monoxide and unconverted fuel. And a third reformate stream 48 containing.

第３リフォーメート流４８は、第２燃料５０と混合され、水素濃縮燃料流５２を形成し、これは、ガスタービンユニット５４に送られる。適宜、第３リフォーメート流４８の一部５８を水素化脱硫（ＨＤＳ）ユニット（６０）に送って、第１燃料１８のＨＤＳ処理に必要とされる水素を供給してもよい。ガスタービンユニット５４は、圧縮機６２、燃焼器６４、ガスタービン６６及び発電機６８を備える。酸化剤７０は、水素濃縮燃料流５２と混合する前に圧縮機６２で圧縮される。圧縮された酸化剤７２と水素濃縮燃料流５２は、燃焼器６４で燃焼され、熱エネルギーと高温圧縮燃焼排気ガス混合物７４を発生し、ガスタービン６６に送られる。圧縮燃焼排ガス混合物７４は膨張してタービンを駆動した後、水蒸気発生器ユニット７８に排気ガス流７６として排出される。ガスタービン排気ガス流７６の一部（７７）はプレ−ＳＭＲ１４に分流され、混合燃料流２８を改質するための熱を供給する。膨張高圧混合ガスによるタービンの回転は、当業者に周知の方法で発電機６８で電力に変換される。   The third reformate stream 48 is mixed with the second fuel 50 to form a hydrogen enriched fuel stream 52 that is sent to the gas turbine unit 54. Optionally, a portion 58 of the third reformate stream 48 may be sent to a hydrodesulfurization (HDS) unit (60) to supply the hydrogen required for HDS processing of the first fuel 18. The gas turbine unit 54 includes a compressor 62, a combustor 64, a gas turbine 66, and a generator 68. The oxidant 70 is compressed by the compressor 62 before being mixed with the hydrogen enriched fuel stream 52. The compressed oxidant 72 and hydrogen enriched fuel stream 52 are combusted in a combustor 64 to generate thermal energy and a hot compressed combustion exhaust gas mixture 74 that is sent to a gas turbine 66. The compressed combustion exhaust gas mixture 74 expands to drive the turbine and is then discharged to the steam generator unit 78 as an exhaust gas stream 76. A portion (77) of the gas turbine exhaust gas stream 76 is diverted to the pre-SMR 14 to provide heat to reform the mixed fuel stream 28. The rotation of the turbine by the expanded high pressure gas mixture is converted to electrical power by the generator 68 in a manner well known to those skilled in the art.

水蒸気発生ユニット７８は、ＨＲＳＧ８０、水蒸気タービン８４及び水蒸気発生器８６を備える。排気ガス７６からの熱を利用して水蒸気２０を発生させるため、ＨＲＳＧ８０は３つのステージ８１、８２及び８３を有する。水蒸気２０を第１燃料１８と合流させて混合燃料流２２を形成する。水蒸気２０は、さらに、プレ−ＳＭＲ１４で改質反応を進行させるとともに、水蒸気タービン８４及び水蒸気発生器８６を介して発電するのにも使用される。水蒸気発生器ユニット７８は、水蒸気タービン出口流９０を凝縮して水流９２を形成するための凝縮器８８をさらに備えていてもよい。水流９２は、水蒸気発生のためにＨＲＳＧ８０にリサイクルしてもよい。冷却排気ガス流９４は環境に排出してもよい。   The steam generation unit 78 includes an HRSG 80, a steam turbine 84, and a steam generator 86. The HRSG 80 has three stages 81, 82, and 83 in order to generate the water vapor 20 using the heat from the exhaust gas 76. Steam 20 is combined with the first fuel 18 to form a mixed fuel stream 22. The steam 20 is further used to cause a reforming reaction in the pre-SMR 14 and to generate power via the steam turbine 84 and the steam generator 86. The steam generator unit 78 may further comprise a condenser 88 for condensing the steam turbine outlet stream 90 to form a water stream 92. The water stream 92 may be recycled to the HRSG 80 for steam generation. The cooled exhaust gas stream 94 may be discharged to the environment.

再度、改質装置ユニット１２について説明すると、プレ−ＳＭＲ１４は従来の水蒸気改質法で第１燃料を改質するように構成されている。しかし、プレ−ＳＭＲは、既存のＳＭＲ改質装置よりも低温で燃料を改質する。従って、以下でさらに詳しく説明する通り、ＮＧ中のメタンは、合成ガス（水素及びＣＯを含む）に部分的にしか転化されない。燃料１８は適当なガス又は液体を含むものであればよい。説明の便宜上、以下、第１燃料１８をＮＧとして説明する。ＮＧとは、主成分のメタンを、様々な量のエタン、プロパン、ブタンその他のガスと共に含む混合ガスをいう。典型的には、ＮＧＣＣシステム１０へのＮＧ供給量の約５〜約５０％をプレ−ＳＭＲ１４に供給できる。具体的には、ＮＧ供給物の約１０〜約３０％、さらに具体的には約２０％がプレ−ＳＭＲ１４で転化される。天然ガスの主成分はメタン（ＣＨ４）であり、これが２段階反応で水蒸気と反応して水素と二酸化炭素とを生成する。図１に示すような技術では、第１の反応はプレ−ＳＭＲ１４で起こり、以下の反応（１）でメタンが水蒸気と反応して水素と一酸化炭素を生成する。 The reformer unit 12 will be described again. The pre-SMR 14 is configured to reform the first fuel by the conventional steam reforming method. However, pre-SMR reforms fuel at a lower temperature than existing SMR reformers. Therefore, as described in more detail below, methane in NG is only partially converted to synthesis gas (including hydrogen and CO). The fuel 18 only needs to contain an appropriate gas or liquid. For convenience of explanation, the first fuel 18 will be described as NG hereinafter. NG refers to a mixed gas containing methane as a main component together with various amounts of ethane, propane, butane and other gases. Typically, about 5 to about 50% of the NG supply to the NGCC system 10 can be supplied to the pre-SMR 14. Specifically, about 10 to about 30%, more specifically about 20% of the NG feed is converted with pre-SMR14. The main component of natural gas is methane (CH 4 ), which reacts with water vapor in a two-stage reaction to produce hydrogen and carbon dioxide. In the technique as shown in FIG. 1, the first reaction occurs in pre-SMR14, and methane reacts with water vapor in the following reaction (1) to generate hydrogen and carbon monoxide.

ＣＨ４＋Ｈ２Ｏ ⇔ ＣＯ＋３Ｈ２ ΔＨｏ ２９８＝＋２５１ｋＪｍｏｌ−１ （１）
水蒸気改質反応（１）は吸熱性である。そのため、水蒸気改質プロセスはエネルギー集約的であり、改質プロセス全体にかなりの熱が必要とされる。上述の通り、プレ−ＳＭＲ１４は、約５００℃〜約８００℃、具体的には約６００℃〜約７００℃、さらに具体的には６５０℃の反応温度で稼動する。第１燃料１８中の炭素の約５０％未満を回収することが望まれるので、プレ−ＳＭＲ１４ではメタンからの水素及び一酸化炭素への約７０％以下の転化効率しか必要とされない。そのため、プレ−ＳＭＲは低温で稼動させることができ、稼動コスト及び高価な耐熱合金がが不要であるので資本コストを削減できる。プレ−ＳＭＲ１４は、吸熱反応（１）の熱を高温ガスタービン排気ガス流からＳＭＲ触媒へと伝達するための多数の管を備えていてもよい。加熱混合燃料流２８は、水蒸気改質用触媒を通して、水素、ＣＯ、ＣＯ２、未転化燃料及び水蒸気の混合物を含む第１リフォーメート流２４へと転化される。次いで、ガスタービン排気ガス流の冷却部分７７は、大気に排出する準備のために排気筒へ送ることができる。プレ−ＳＭＲ触媒は、当業者に公知の従来のＳＭＲ触媒、例えばニッケル系触媒などでよい。適宜、改質装置ユニット１２は、第１燃料１８に水蒸気２０を混合するために好適な供給原料サチュレータ回路をさらに備えていてもよい。 CH 4 + H 2 O⇔CO + 3H 2 ΔH o 298 = + 251 kJmol −1 (1)
The steam reforming reaction (1) is endothermic. As such, the steam reforming process is energy intensive and requires significant heat throughout the reforming process. As described above, the pre-SMR 14 operates at a reaction temperature of about 500 ° C. to about 800 ° C., specifically about 600 ° C. to about 700 ° C., more specifically 650 ° C. Since it is desired to recover less than about 50% of the carbon in the first fuel 18, the pre-SMR 14 requires less than about 70% conversion efficiency from methane to hydrogen and carbon monoxide. Therefore, the pre-SMR can be operated at a low temperature, and the capital cost can be reduced since the operation cost and the expensive heat-resistant alloy are unnecessary. The pre-SMR 14 may comprise a number of tubes for transferring the heat of the endothermic reaction (1) from the hot gas turbine exhaust gas stream to the SMR catalyst. The heated mixed fuel stream 28 is converted through a steam reforming catalyst into a first reformate stream 24 comprising a mixture of hydrogen, CO, CO 2 , unconverted fuel and steam. The cooling portion 77 of the gas turbine exhaust gas stream can then be sent to the exhaust stack in preparation for venting to the atmosphere. The pre-SMR catalyst may be a conventional SMR catalyst known to those skilled in the art, such as a nickel-based catalyst. Optionally, the reformer unit 12 may further include a feedstock saturator circuit suitable for mixing the first fuel 18 with the water vapor 20.

第１リフォーメート流２４を適宜熱交換器１６で冷却した後、冷却第１リフォーメート流２６は転化反応ユニット３０に入る。水蒸気改質プロセスの第２反応がＷＧＳ反応器３２中で起こり、冷却第１リフォーメート流２６の中のＣＯ及び水蒸気は以下の反応（２）でＣＯ２と水素に転化される。 After the first reformate stream 24 is appropriately cooled by the heat exchanger 16, the cooled first reformate stream 26 enters the conversion reaction unit 30. The second reaction of the steam reforming process takes place in the WGS reactor 32 and the CO and steam in the cooled first reformate stream 26 are converted to CO 2 and hydrogen in the following reaction (2).

ＣＯ＋Ｈ２Ｏ ⇔ ＣＯ２＋Ｈ２ ΔＨ＝−４１．１６ｋＪ／ｍｏｌ （２）
シフト反応（２）は穏やかに発熱し、転化触媒の存在下で起こる。従って、第１リフォーメート流２６は、反応の進行に伴って触媒層を横切る温度が上昇する。転化触媒としては、高温転化触媒（ＨＴＳ）又は低温転化触媒（ＬＴＳ）又はＨＴＳとＬＴＳ触媒との組合せが挙げられる。ＷＧＳ反応器３２における反応温度は２００℃〜約６００℃である。ただし、低温に維持すると反応（２）が右にずれて、水素とＣＯ２の発生量が増し、水蒸気とＣＯの生成量が減る。したがって、ＷＧＳ反応器は約３００℃〜約４００℃の温度域、さらに具体的には約３５０℃で稼動できる。第１リフォーメート流２６のＣＯ２及び水素への転化は、第２リフォーメート流３４を生じる。さらに、改質装置ユニット１２及び転化反応ユニット３０は、（図１に示すように）装置の別個の部分でもよいし、プレ−ＳＭＲ１４及びＷＧＳ反応器３２の両方を含む装置の単一部分でもよい。 CO + H 2 O⇔CO 2 + H 2 ΔH = −41.16 kJ / mol (2)
Shift reaction (2) is mildly exothermic and takes place in the presence of a conversion catalyst. Accordingly, the temperature of the first reformate stream 26 across the catalyst layer increases as the reaction proceeds. Conversion catalysts include high temperature conversion catalyst (HTS), low temperature conversion catalyst (LTS), or a combination of HTS and LTS catalyst. The reaction temperature in the WGS reactor 32 is 200 ° C. to about 600 ° C. However, if maintained at a low temperature, the reaction (2) shifts to the right, the generation amounts of hydrogen and CO 2 increase, and the generation amounts of water vapor and CO decrease. Thus, the WGS reactor can be operated in a temperature range of about 300 ° C. to about 400 ° C., more specifically about 350 ° C. Conversion of the first reformate stream 26 to CO 2 and hydrogen results in a second reformate stream 34. Further, the reformer unit 12 and the conversion reaction unit 30 may be separate parts of the apparatus (as shown in FIG. 1) or a single part of the apparatus that includes both the pre-SMR 14 and the WGS reactor 32.

二酸化炭素除去ユニット４０は、アミン吸収塔４２及び再生塔４４を備えていてもよい。第２リフォーメート流３４は、アミンを用いたＣＯ２の化学吸収を促進するため熱交換器３６で適当な温度に冷却してもよい。この技術は、比較的に低温でＣＯ２を吸収でき、リッチソルベントの昇温によって容易に再生できるアルカノールアミン溶媒に基づく。この技術で使用される溶媒としては、例えばトリエタノールアミン、モノエタノールアミン、ジエタノールアミン、ジイソプロパノールアミン、ジグリコールアミン、メチルジエタノールアミンなどが挙げられる。上述の通り、回収ＣＯ２は、第１燃料１８中の炭素の約５０％未満とし得る。年間ＣＯ２排出割当量を超える排出量についてのペナルティ税を避けるのに十分なＣＯ２が回収される。しかし、完全なＣＯ２回収を有する従来技術のシステムに比べて、本発明のシステムでは、資本投下及び運転費用が低減し、エネルギー効率は増す。こうして生成・回収したＣＯ２流４６は、所望の場所に容易に輸送できる。例えば、ＣＯ２は、貯蔵（隔離）に適した地下構造物或いは原油増進回収法（ＥＯＲ）のため油田に注入できる場所、或いは製造プロセスに使用される場所に輸送すればよい。 The carbon dioxide removal unit 40 may include an amine absorption tower 42 and a regeneration tower 44. The second reformate stream 34 may be cooled to a suitable temperature by a heat exchanger 36 to promote chemical absorption of CO 2 using amines. This technique is based on alkanolamine solvents that can absorb CO 2 at relatively low temperatures and can be easily regenerated by increasing the temperature of the rich solvent. Examples of the solvent used in this technique include triethanolamine, monoethanolamine, diethanolamine, diisopropanolamine, diglycolamine, and methyldiethanolamine. As described above, the recovered CO 2 may be less than about 50% of the carbon in the first fuel 18. Sufficient CO 2 is recovered to avoid penalties for emissions that exceed the annual CO 2 emission quota. However, compared to prior art systems with complete CO 2 capture, the system of the present invention reduces capital investment and operating costs and increases energy efficiency. The CO 2 stream 46 thus produced and recovered can be easily transported to a desired location. For example, CO 2 may be transported to an underground structure suitable for storage (sequestration) or to a location where it can be injected into an oil field for enhanced oil recovery (EOR) or used in a manufacturing process.

二酸化炭素除去ユニット４０からの残存流は、主に水素、ＣＯ、未利用燃料及び水を含む第３リフォーメート流４８である。この流れは、燃焼のためガスタービンユニット５４に送られる。適宜、この流れの一部５８をＨＤＳユニット６０に送ってもよい。ＨＤＳユニット６０で、第１燃料１８に含まれる硫黄は、ＨＤＳユニット６０の脱硫カラムの水添脱硫器によって硫化水素に転化される。硫化水素は次いでＨＤＳユニット６０の脱硫カラム下流の硫黄吸収器又は吸着ユニットで吸着・除去される。硫黄は、プレ−ストリーム改質触媒を被毒しかねないので、第１燃料１８から硫黄を除去するのが有利である。ＨＤＳプロセスに必要とされる水素は、独立した水素源の流れを必要とせず、第３リフォーメート流４８の一部５８を分流することによって、閉ループサイクルで供給される。ＨＤＳユニット６０は、約２００℃〜約４００℃、具体的には約２５０℃〜約３５０℃の温度で稼動できる。ＨＤＳプロセスで用いる触媒は、既存のＨＤＳ触媒、例えばＳｕｄ Ｃｈｅｍｉｅ社又はＨａｌｄｏｒ Ｔｏｐｓｏｅ社から市販のもの、例えばコバルト及びモリブデンの硫化物、或いはニッケル及びモリブデンでよい。   The remaining stream from the carbon dioxide removal unit 40 is a third reformate stream 48 that mainly contains hydrogen, CO, unused fuel and water. This stream is sent to the gas turbine unit 54 for combustion. A part 58 of this flow may be sent to the HDS unit 60 as appropriate. In the HDS unit 60, sulfur contained in the first fuel 18 is converted into hydrogen sulfide by the hydrodesulfurizer of the desulfurization column of the HDS unit 60. The hydrogen sulfide is then adsorbed and removed by a sulfur absorber or adsorption unit downstream of the HDS unit 60 desulfurization column. Because sulfur can poison the pre-stream reforming catalyst, it is advantageous to remove sulfur from the first fuel 18. The hydrogen required for the HDS process is supplied in a closed loop cycle by diverting a portion 58 of the third reformate stream 48 without requiring a separate hydrogen source stream. The HDS unit 60 can operate at a temperature of about 200 ° C. to about 400 ° C., specifically about 250 ° C. to about 350 ° C. The catalyst used in the HDS process may be an existing HDS catalyst, such as those commercially available from Sud Chemie or Haldor Topsoe, such as cobalt and molybdenum sulfides, or nickel and molybdenum.

第３リフォーメート流４８と第２燃料５０は、ガスタービンユニット５４に入る前に、混合されて水素濃縮燃料流５２を形成する。第２燃料は、発電システム１０に送られた燃料、すなわちＮＧの残りを含む。典型的に、ＮＧＣＣシステム１０へのＮＧ供給物の約５０〜約９５％はガスタービンユニット５４の燃料として消費し得る。特にＮＧ供給物の約７０〜約９０％、さらに具体的に約８０％が燃焼器６４で消費され、複合サイクルプラントの全ＣＯ２の約１０％を回収できる。水素濃縮燃料流５２は燃焼器６４に噴射されて、圧縮酸化剤７２の存在下で燃焼し、高温圧縮燃焼排ガス混合物７４を生ずる。水素濃縮燃料は、第２燃料５０単独の使用に比べて、燃焼器６４内での火炎安定性を拡げ、燃焼はより希薄（リーン）であり、火炎温度を低くできる。この結果、燃焼器６４中の低い火炎温度により、燃焼器排気ガスの窒素酸化物排出量は低減する。また、燃焼器は、第２燃料５０だけを用いる燃焼器に比べて、さらにターンダウンできる能力をもつ。さらに、天然ガスに水素を添加することによって、発電と同時に低い排出を維持するための燃焼器の動作可能ウインドウが拡大する。高温圧縮混合ガス７４は燃焼器６４を出て、ガスタービン６６を通り、そこで高温圧縮混合ガス７４が部分的に冷却及び膨張して機械力を発生する。機械力は発電装置６８で電力に変換される。膨張して部分的に冷却された排気ガス７６はガスタービン６６を出て、水蒸気発生器ユニット７８に入る。 The third reformate stream 48 and the second fuel 50 are mixed to form a hydrogen enriched fuel stream 52 before entering the gas turbine unit 54. The second fuel includes the fuel sent to the power generation system 10, that is, the remainder of NG. Typically, about 50 to about 95% of the NG supply to the NGCC system 10 may be consumed as fuel for the gas turbine unit 54. In particular, about 70 to about 90%, more specifically about 80%, of the NG feed is consumed by the combustor 64, and about 10% of the total CO 2 of the combined cycle plant can be recovered. The hydrogen enriched fuel stream 52 is injected into the combustor 64 and combusts in the presence of the compressed oxidant 72 to produce a hot compressed flue gas mixture 74. Compared with the use of the second fuel 50 alone, the hydrogen-enriched fuel expands the flame stability in the combustor 64, and the combustion is leaner, and the flame temperature can be lowered. As a result, the low flame temperature in the combustor 64 reduces the nitrogen oxide emissions of the combustor exhaust gas. Further, the combustor has the ability to be further turned down as compared with the combustor using only the second fuel 50. Furthermore, adding hydrogen to natural gas expands the combustor operable window to maintain low emissions simultaneously with power generation. The hot compressed gas mixture 74 exits the combustor 64 and passes through a gas turbine 66 where the hot compressed gas mixture 74 is partially cooled and expanded to generate mechanical force. The mechanical force is converted into electric power by the power generation device 68. The expanded and partially cooled exhaust gas 76 exits the gas turbine 66 and enters the steam generator unit 78.

水蒸気発生器ユニット７８はＨＲＳＧ８０を備えており、排気ガス７６から廃熱を回収して水蒸気２０を発生させる。ＨＲＳＧ８０は排気ガス７６を冷却し、水蒸気２０を生成するための３つのステージ８１、８２及び８３を有する。水蒸気２０の一部は水蒸気タービン８４に送られ、そこで水蒸気２０が膨張及び冷却して機械力を発生する。この機械力は発電装置８６で電力に変換される。膨張して冷却された水蒸気はタービン８４を出て、凝縮器８８でさらに冷却・凝縮して、ＨＲＳＧ８０に導入される水流９２を形成する。次いで冷却排気ガス９４は、大気中に排出のために排気筒に送られる。上述の通り、水蒸気２０の残りは第１燃料１８と合流して混合燃料流２２を形成し、次いでプレ−ＳＭＲ１４へ送られる。プレ−ＳＭＲ１４に水蒸気２０の残りを送ると、好都合なことに、リフォーメーション反応の進行に必要な水蒸気を供給するための追加の水蒸気発生器をシステム１０が有している必要がなくなる。   The steam generator unit 78 includes an HRSG 80 and recovers waste heat from the exhaust gas 76 to generate steam 20. The HRSG 80 has three stages 81, 82 and 83 for cooling the exhaust gas 76 and generating the water vapor 20. A portion of the steam 20 is sent to the steam turbine 84 where the steam 20 expands and cools to generate mechanical force. This mechanical force is converted into electric power by the power generator 86. The expanded and cooled water vapor exits the turbine 84 and further cools and condenses in the condenser 88 to form a water stream 92 that is introduced into the HRSG 80. The cooled exhaust gas 94 is then sent to the exhaust stack for discharge into the atmosphere. As described above, the remainder of the water vapor 20 merges with the first fuel 18 to form a mixed fuel stream 22 that is then sent to the pre-SMR 14. Sending the remainder of the water vapor 20 to the pre-SMR 14 advantageously eliminates the need for the system 10 to have an additional water vapor generator to supply the water vapor necessary for the reforming reaction to proceed.

次いで図２を参照すると、第２の例示的な発電システム１００を例示する。図１の第１の実施形態と共通の要素についての説明は省略した。   Referring now to FIG. 2, a second exemplary power generation system 100 is illustrated. A description of elements common to the first embodiment in FIG. 1 is omitted.

図２で、ＨＲＳＧ８０の第１ステージ８１（図１に示す）はプレ−ＳＭＲ９６である。図２の発電システム１００は、水蒸気発生器ユニット７８（図１）を改質装置ユニット１２（図１）と組み合わせて複合ユニット９８を形成する。ＨＲＳＧ８０の第１ステージ９６は、プレ−ＳＭＲとして機能するように改造される。ＨＲＳＧ８０は、シェルチューブ型熱交換器とし得る。その場合、プレ−ＳＭＲ触媒は、ＨＲＳＧ８０の第１ステージのチューブ側（低温側）に充填できる。排気ガス７６は、ＨＲＳＧ８０の第１ステージ９６のシェル側（高温側）に通せばよい。第１ステージ９６は、約６００℃〜約９００℃の温度域で稼動するように構成される。予熱混合燃料流２８は、第１の実施形態で説明した通り、第１ステージ９６のチューブ内のプレ−ＳＭＲ触媒を通過して燃料を改質し、第１リフォーメート流２４を生成する。第１ステージ９６のシェル側を流れる高温ガスタービン排気ガス７６は、上述の通り、吸熱水蒸気改質反応（１）の進行に必要な熱を供給する。ＨＲＳＧ８０の残りのステージ８２及び８３は、水９２に排気ガス７６中の熱の残りを伝達し、水蒸気２０を生成する。適宜、熱を第１リフォーメート流２４から混合燃料流２２に伝達するための複合ユニット９８の部分として、熱交換器１６を備えていてもよい。   In FIG. 2, the first stage 81 (shown in FIG. 1) of the HRSG 80 is a pre-SMR 96. The power generation system 100 of FIG. 2 forms a composite unit 98 by combining the steam generator unit 78 (FIG. 1) with the reformer unit 12 (FIG. 1). The first stage 96 of the HRSG 80 is modified to function as a pre-SMR. The HRSG 80 may be a shell tube heat exchanger. In that case, the pre-SMR catalyst can be filled on the tube side (low temperature side) of the first stage of the HRSG 80. The exhaust gas 76 may be passed through the shell side (high temperature side) of the first stage 96 of the HRSG 80. The first stage 96 is configured to operate in a temperature range of about 600 ° C to about 900 ° C. As described in the first embodiment, the preheated mixed fuel stream 28 passes through the pre-SMR catalyst in the tube of the first stage 96 to reform the fuel and generate a first reformate stream 24. As described above, the high-temperature gas turbine exhaust gas 76 flowing on the shell side of the first stage 96 supplies heat necessary for the progress of the endothermic steam reforming reaction (1). The remaining stages 82 and 83 of the HRSG 80 transfer the remainder of the heat in the exhaust gas 76 to the water 92 and produce water vapor 20. Optionally, a heat exchanger 16 may be provided as part of the composite unit 98 for transferring heat from the first reformate stream 24 to the mixed fuel stream 22.

ＨＲＳＧ８０の第１ステージ９６をプレ−ＳＭＲに改造することによって、本発明の部分的ＣＯ２回収式ＮＧＣＣ発電システムに要する資本費が減る。別個のプレ−ＳＭＲの建造コストが節約され、かかるユニットの設置に必要な空間も同様に節約される。さらに、大半の発電プラントがＨＲＳＧを含むので、これらのユニットがプレ−ＳＭＲステージを備えるように改造することができ、既存のＮＧＣＣプラントで本発明の部分的ＣＯ２回収システムの低コストの利点を得るのに、既存の発電プラントの改造に必要な費用及び空間を削減できる。 By modifying the first stage 96 of the HRSG 80 to pre-SMR, the capital cost required for the partial CO 2 capture NGCC power generation system of the present invention is reduced. The cost of building a separate pre-SMR is saved, as well as the space required to install such a unit. In addition, since most power plants include HRSG, these units can be retrofitted to include a pre-SMR stage, providing the low cost benefits of the partial CO 2 capture system of the present invention in an existing NGCC plant. In addition, the cost and space required for retrofitting existing power plants can be reduced.

上述の通り、本発明のシステムで用いる燃料は好ましくはＮＧを含む。ただし、本システムでは、例えばバイオガス（主にメタンを含む）、ＬＰガス（ＬＰＧ）、ナフサ、ブタン、プロパン、ディーゼル、灯油、エタノール、メタノール、航空燃料、石炭誘導燃料、バイオ燃料、含酸素炭化水素原料及びこれらの混合物などのいかなる好適なガス又は液体も燃料として使用できるように構成してもよい。第１燃料１８及び第２燃料５０のいずれも、各々本明細書に記載したこれらの燃料の具体例から選択できる。一実施形態では、第１燃料１８及び第２燃料５０は同じである。本発明のシステムで用いる酸化剤７０は、酸素を含むガス、例えば空気、酸素リッチ空気、低酸素空気、空気分離ユニット（ＡＳＵ）からの酸素などを含むことができる。   As mentioned above, the fuel used in the system of the present invention preferably contains NG. However, in this system, for example, biogas (mainly including methane), LP gas (LPG), naphtha, butane, propane, diesel, kerosene, ethanol, methanol, aviation fuel, coal-derived fuel, biofuel, oxygenated carbonization Any suitable gas or liquid such as a hydrogen feed and mixtures thereof may be configured to be used as fuel. Each of the first fuel 18 and the second fuel 50 can be selected from the specific examples of these fuels described herein. In one embodiment, the first fuel 18 and the second fuel 50 are the same. The oxidant 70 used in the system of the present invention can include a gas containing oxygen, such as air, oxygen rich air, low oxygen air, oxygen from an air separation unit (ASU), and the like.

本明細書に記載したＮＧＣＣ発電システムは、多くの利点を有する。部分的メタン転化用に構築された低温・低コストプレ−ＳＭＲユニットをシステムに組み込むことによって、メタンの完全転化用に構築された完全なＳＭＲ改質装置を用いるシステムに比べて、燃料コスト、資本コスト及びエネルギーコストを削減できる。同様に、資本及びエネルギーコストは、燃料流の全炭素含有量を回収するのとは対照的に、ＣＯ２の一部（炭素税を避けるのに必要な回収量）だけを回収することによって削減される。また、好適に配置された熱交換器の使用及びシステム全体のリサイクルループは全体的効率を向上させる。さらに、本発明の部分的ＣＯ２回収式ＮＧＣＣシステムは、既存のＮＧＣＣ発電プラントを改造して組み込むことができ、排出量を低減して排出ペナルティ又は炭素税を回避することができる。本発明のシステムの低温での稼動及び小さいサイズは、これらが、大きな資本投下なしで、最小不動産しか有していない既存のプラントに組み込むことができることを意味している。 The NGCC power generation system described herein has many advantages. By incorporating a low temperature, low cost pre-SMR unit built for partial methane conversion into the system, fuel costs and capital costs compared to a system using a complete SMR reformer built for full methane conversion And energy costs can be reduced. Similarly, capital and energy costs are reduced by recovering only a portion of CO 2 (recovery necessary to avoid carbon tax) as opposed to recovering the total carbon content of the fuel stream. Is done. Also, the use of suitably arranged heat exchangers and the overall system recycle loop improves overall efficiency. Furthermore, the partial CO 2 capture NGCC system of the present invention can be retrofitted into an existing NGCC power plant to reduce emissions and avoid emission penalties or carbon taxes. The low temperature operation and small size of the system of the present invention means that they can be incorporated into existing plants that have minimal real estate without significant capital investment.

本発明を例示的な実施形態に関して説明してきたが、本発明の範囲から逸脱することなしに様々な変更が多分なされるであろうし、均等物でこの要素を置換し得ることは、当業者によって理解されるであろう。さらに、多くの改変が、本発明の必須の範囲を逸脱することなく、発明の教示に特定の状況又は材料を適応させるように行うことができる。従って、本発明は、本発明を実施するために考えられる最良の形態として本発明の特定の実施形態に限定されず、付属する特許請求の範囲に入るすべての実施形態を含むであろうということが意図されている。   Although the present invention has been described in terms of exemplary embodiments, it will be appreciated by those skilled in the art that various changes may be made without departing from the scope of the present invention, and equivalent elements may be substituted. Will be understood. In addition, many modifications may be made to adapt a particular situation or material to the teachings of the invention without departing from the essential scope of the invention. Accordingly, the invention is not limited to the specific embodiments of the invention as the best mode contemplated for carrying out the invention, but will include all embodiments that fall within the scope of the appended claims. Is intended.

例示的な部分的ＣＯ２回収式複合サイクル発電システムの概略図。1 is a schematic diagram of an exemplary partial CO 2 capture combined cycle power generation system. FIG. 別の例示的な部分的ＣＯ２回収式複合サイクル発電システムの概略図。FIG. 3 is a schematic diagram of another exemplary partial CO 2 capture combined cycle power generation system.

符号の説明Explanation of symbols

１０ ＮＧＣＣ発電システム
１２ 改質装置ユニット
１４ プレ−水蒸気−メタン改質装置
１６ 熱交換器
１８ 第１燃料
２０ 水蒸気
２２ 混合燃料流
２４ 第１リフォーメート流
２６ 冷却第１リフォーメート流
２８ 加熱混合燃料流
３０ 転化反応ユニット
３２ 水−ガス−転化反応器
３４ 第２リフォーメート流
３６ 熱交換器
３８ 冷却第２リフォーメート流
４０ 二酸化炭素除去ユニット
４２ アミン吸収塔
４４ 再生塔
４８ 第３リフォーメート流
５０ 第２燃料
５２ 水素濃縮燃料流
５４ ガスタービンユニット
５８ 部分
６０ 水素化脱硫ユニット
６２ 圧縮機
６４ 燃焼器
６６ ガスタービン
６８ 発電装置
７０ 酸化剤
７２ 圧縮酸化剤
７４ 排気ガス混合物
７６ ガスタービン排気ガス流
７７ 部分
７８ 水蒸気発生器ユニット
８０ 熱回収水蒸気発生器
８１ 第１ステージ
８２ 第２ステージ
８３ 第３ステージ
８４ 水蒸気タービン
８６ 水蒸気発生器
８８ 凝縮器
９０ 水蒸気タービン排出流
９２ 水流
９４ 冷却排気ガス流
９６ プレ−水蒸気−メタン−改質装置
９８ 複合ユニット
１００ 複合サイクル発電システム DESCRIPTION OF SYMBOLS 10 NGCC power generation system 12 Reformer unit 14 Pre-steam-methane reformer 16 Heat exchanger 18 First fuel 20 Steam 22 Mixed fuel stream 24 First reformate stream 26 Cooling first reformate stream 28 Heated mixed fuel stream 30 Conversion reaction unit 32 Water-gas-conversion reactor 34 Second reformate stream 36 Heat exchanger 38 Cooled second reformate stream 40 Carbon dioxide removal unit 42 Amine absorption tower 44 Regeneration tower 48 Third reformate stream 50 Second Fuel 52 Hydrogen-enriched fuel stream 54 Gas turbine unit 58 Part 60 Hydrodesulfurization unit 62 Compressor 64 Combustor 66 Gas turbine 68 Power generator 70 Oxidant 72 Compressed oxidant 74 Exhaust gas mixture 76 Gas turbine exhaust gas stream 77 Part 78 Steam Generator unit 80 Heat recovery Steam generator 81 First stage 82 Second stage 83 Third stage 84 Steam turbine 86 Steam generator 88 Condenser 90 Steam turbine exhaust stream 92 Water stream 94 Cooling exhaust gas stream 96 Pre-steam-methane-reformer 98 Combined unit 100 Combined cycle power generation system

Claims (10)

複合サイクルシステム（１０，１００）であって、
約８００℃未満の温度で稼動して、第１燃料（１８）と水蒸気（２０）とを含む混合燃料流（２２）を改質して第１リフォーメート流（２４）を生成するように構成されたプレ−水蒸気−メタン−改質装置（１４，９６）を備える改質装置ユニット（１２）、
第１リフォーメート流中の一酸化炭素を二酸化炭素に転化させて第２リフォーメート流（３４）を生成するように構成された水−ガス−転化反応器（３２）を備える転化反応ユニット（３０）、
第２リフォーメート流から二酸化炭素を除去して二酸化炭素流（４６）と第３リフォーメート流（４８）とを生成するように構成された二酸化炭素除去ユニット（４０）であって、第１燃料中に含まれる炭素の約５０％未満を二酸化炭素として回収する二酸化炭素除去ユニット（４０）、
第３リフォーメートと第２燃料（５０）との混合物を受け入れて電力及び排気ガス流（７４）を発生するように構成されたガスタービンユニット（５４）であって、排気ガス流が混合燃料流を改質するための熱を供給するガスタービンユニット（５４）、及び
排気ガス流を受け入れるように構成された水蒸気発生器ユニット（７８）であって、排気ガス流の熱を水流（９２）に伝達して冷却排気ガス流（９４）及び水蒸気タービンのための水蒸気（８４）及び混合燃料流を生成する水蒸気発生器ユニット（７８）
を備える複合サイクルシステム（１０，１００）。 A combined cycle system (10,100),
Operated at a temperature less than about 800 ° C. and configured to reform a mixed fuel stream (22) comprising a first fuel (18) and water vapor (20) to produce a first reformate stream (24). Reformer unit (12) comprising an improved pre-steam-methane-reformer (14, 96),
A conversion reaction unit (30) comprising a water-gas conversion reactor (32) configured to convert carbon monoxide in the first reformate stream to carbon dioxide to produce a second reformate stream (34). ),
A carbon dioxide removal unit (40) configured to remove carbon dioxide from a second reformate stream to produce a carbon dioxide stream (46) and a third reformate stream (48), the first fuel A carbon dioxide removal unit (40) for recovering less than about 50% of the carbon contained therein as carbon dioxide,
A gas turbine unit (54) configured to receive a mixture of a third reformate and a second fuel (50) to generate electric power and an exhaust gas stream (74), wherein the exhaust gas stream is a mixed fuel stream. A gas turbine unit (54) for supplying heat for reforming the steam, and a steam generator unit (78) configured to receive an exhaust gas stream, wherein the heat of the exhaust gas stream is converted to a water stream (92) A steam generator unit (78) that communicates to produce a cooled exhaust gas stream (94) and a steam (84) and mixed fuel stream for the steam turbine
A combined cycle system (10,100) comprising: 水蒸気発生器ユニット（７８）が、２以上のステージ（８１，８２）を含む熱回収水蒸気発生器（８０）を備えていて、１つのステージ（８１）がプレ−水蒸気−メタン−改質装置（９６）を備えており、該プレ−水蒸気−メタン−改質装置で、排気ガス流からの熱を利用して混合燃料流を改質する、請求項１記載の複合サイクルシステム。 The steam generator unit (78) includes a heat recovery steam generator (80) including two or more stages (81, 82), and one stage (81) is a pre-steam-methane-reformer ( 96), wherein the pre-steam-methane-reformer utilizes the heat from the exhaust gas stream to reform the mixed fuel stream. 改質装置ユニットが、第１リフォーメート流及び混合燃料流を受け入れるように構成された熱交換器（１６）であって、第１リフォーメート流からの熱を混合流に伝達して冷却第１リフォーメート流（２６）と加熱混合燃料流（２８）とを生成し、加熱混合燃料流をプレ−水蒸気−メタン−改質装置に送る熱交換器（１６）をさらに備える、請求項１記載の複合サイクルシステム。 A reformer unit is a heat exchanger (16) configured to receive a first reformate stream and a mixed fuel stream, wherein the reformer unit transfers heat from the first reformate stream to the mixed stream for cooling first. The heat exchanger (16) of claim 1, further comprising a heat exchanger (16) for generating a reformate stream (26) and a heated mixed fuel stream (28) and sending the heated mixed fuel stream to a pre-steam-methane-reformer. Combined cycle system. 転化反応ユニット（３０）が、第２リフォーメート流及び第１燃料を受け入れるように構成された熱交換器（３６）であって、第２リフォーメート流からの熱を第１燃料に伝達して冷却第２リフォーメート流（３８）と加熱第１燃料とを生成する熱交換器（３６）をさらに備える、請求項１記載の複合サイクルシステム。 A conversion reaction unit (30) is a heat exchanger (36) configured to receive the second reformate stream and the first fuel, transferring heat from the second reformate stream to the first fuel. The combined cycle system of any preceding claim, further comprising a heat exchanger (36) that produces a cooled second reformate stream (38) and a heated first fuel. 当該複合サイクルシステムが、第１燃料（１８）を受け入れるように構成された水素化脱硫ユニット（６０）をさらに備えており、第３リフォーメート流（４８）の一部を第１燃料（１８）と合流させて水素化脱硫ユニット（６０）に送る、請求項４記載の複合サイクルシステム。 The combined cycle system further comprises a hydrodesulfurization unit (60) configured to receive the first fuel (18), wherein a portion of the third reformate stream (48) is part of the first fuel (18). The combined cycle system according to claim 4, wherein the combined cycle system is fed to the hydrodesulfurization unit (60). 改質ユニット（１２）が約７０％以下のメタン転化率を有する、請求項１記載の複合サイクルシステム。 The combined cycle system of claim 1, wherein the reforming unit (12) has a methane conversion of about 70% or less. 部分的に二酸化炭素を回収して発電する方法であって、
プレ−水蒸気−メタン−改質装置（１４，９６）で、約８００℃未満の温度で、第１燃料（１８）と水蒸気（２０）とを含む混合燃料流（２２）を改質して水素と一酸化炭素と水蒸気とを含む第１リフォーメート流（２４）を生成させ、
水−ガス転化反応器（３２）で、水蒸気及び第１リフォーメート流中の一酸化炭素を、二酸化炭素と水素とを含む第２リフォーメート流（３４）に転化させ、
二酸化炭素除去ユニット（４０）で、第２リフォーメート流から二酸化炭素を除去して二酸化炭素流（４６）と第３リフォーメート流（４８）とを生成させ、第１燃料中に含まれる炭素の約５０％未満を二酸化炭素除去ユニットで二酸化炭素として回収し、
ガスタービンユニット（５４）で、第３リフォーメート流と第２燃料流（５０）との混合物を燃焼させて電力を発生させ、排気ガス流（７６）を生成させ、
熱回収水蒸気発生器（８０）で、排気ガス流中の熱を利用して水蒸気を発生させ、水蒸気で電力を発生させるとともに第１燃料（１８）との混合燃料流（２２）を生成させる
ことを含んでなる方法。 A method for generating electricity by partially recovering carbon dioxide,
A pre-steam-methane-reformer (14,96) reforms the mixed fuel stream (22) containing the first fuel (18) and steam (20) at a temperature below about 800 ° C. to produce hydrogen. Producing a first reformate stream (24) comprising carbon monoxide and water vapor;
In a water-gas conversion reactor (32), steam and carbon monoxide in the first reformate stream are converted to a second reformate stream (34) comprising carbon dioxide and hydrogen;
In the carbon dioxide removal unit (40), carbon dioxide is removed from the second reformate stream to generate a carbon dioxide stream (46) and a third reformate stream (48), and the carbon contained in the first fuel Less than about 50% is recovered as carbon dioxide in the carbon dioxide removal unit,
In the gas turbine unit (54), a mixture of the third reformate stream and the second fuel stream (50) is burned to generate electric power, and an exhaust gas stream (76) is generated.
A heat recovery steam generator (80) generates steam using heat in the exhaust gas stream to generate electric power with the steam and generate a mixed fuel stream (22) with the first fuel (18). Comprising a method. 改質が、熱回収水蒸気発生器（８０）でも行われ、熱回収水蒸気発生器が２以上のステージ（８１，８２）を含んでいて、１つのステージ（８１）がプレ−水蒸気−メタン−改質装置（９６）を備えており、該プレ−水蒸気−メタン−改質装置で、排気ガス流からの熱を利用して混合燃料流（２２）を改質して第１リフォーメート流（２４）を生成させる、請求項７記載の方法。 The reforming is also performed in the heat recovery steam generator (80), the heat recovery steam generator includes two or more stages (81, 82), and one stage (81) is pre-steam-methane-modified. And the first reformate stream (24) using the pre-steam-methane-reformer to reform the mixed fuel stream (22) using heat from the exhaust gas stream. ) Is generated. 熱交換器で、熱を第１リフォーメート流から混合燃料流に伝達して、冷却第１リフォーメート流と前加熱混合燃料流とを生成し、加熱混合燃料流をプレ−水蒸気−メタン−改質装置に送る、請求項７記載の方法。 In the heat exchanger, heat is transferred from the first reformate stream to the mixed fuel stream to produce a cooled first reformate stream and a preheated mixed fuel stream, and the heated mixed fuel stream is pre-steam-methane-modified. The method of claim 7, wherein the method is sent to a quality device. 熱交換器で、熱を第２リフォーメート流から第１燃料に伝達して、冷却第２リフォーメート流と加熱第１燃料とを生成する、請求項７記載の方法。 8. The method of claim 7, wherein heat is transferred from the second reformate stream to the first fuel in a heat exchanger to produce a cooled second reformate stream and a heated first fuel.
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